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1.
《Applied Geochemistry》2000,15(7):1003-1018
Stream discharges and concentrations of dissolved and colloidal metals (Al, Ca, Cu, Fe, Mg, Mn, Pb, and Zn), SO4, and dissolved silica were measured to identify chemical transformations and determine mass transports through two mixing zones in the Animas River that receive the inflows from Cement and Mineral Creeks. The creeks were the dominant sources of Al, Cu, Fe, and Pb, whereas the upstream Animas River supplied about half of the Zn. With the exception of Fe, which was present in dissolved and colloidal forms, the metals were dissolved in the acidic, high-SO4 waters of Cement Creek (pH 3.8). Mixing of Cement Creek with the Animas River increased pH to near-neutral values and transformed Al and some additional Fe into colloids which also contained Cu and Pb. Aluminium and Fe colloids had already formed in the mildly acidic conditions in Mineral Creek (pH 6.6) upstream of the confluence with the Animas River. Colloidal Fe continued to form downstream of both mixing zones. The Fe- and Al-rich colloids were important for transport of Cu, Pb, and Zn, which appeared to have sorbed to them. Partitioning of Zn between dissolved and colloidal phases was dependent on pH and colloid concentration. Mass balances showed conservative transports for Ca, Mg, Mn, SO4, and dissolved silica through the two mixing zones and small losses (<10%) of colloidal Al, Fe and Zn from the water column.  相似文献   

2.
《Applied Geochemistry》1995,10(3):285-306
Inflows of metal-rich, acidic water that drain from mine dumps and tailings piles in the Leadville, Colorado, area enter the non-acidic water in the upper Arkansas River. Hydrous iron oxides precipitate as colloids and move downstream in suspension, particularly downstream from California Gulch, which has been the major source of metal loads. The colloids influence the concentrations of metals dissolved in the water and the concentrations in bed sediments. To determine the role of colloids, samples of water, colloids, and fine-grained bed sediment were obtained at stream-gaging sites on the upper Arkansas River and at the mouths of major tributaries over a 250-km reach. Dissolved and colloidal metal concentrations in the water column were operationally defined using tangential-flow filtration through 0.001-pm membranes to separate the water and the colloids. Surface-extractable and total bed sediment metal concentrations were obtained on the <60-μm fraction of the bed sediment. The highest concentrations of metals in water, colloids, and bed sediments occurred just downstream from California Gulch. Iron dominated the colloid composition, but substantial concentrations of As, Cd, Cu, Mn, Pb, and Zn also occurred in the colloidal solids. The colloidal load decreased by one half in the first 50 km downstream from the mining inflows due to sedimentation of aggregated colloids to the streambed. Nevertheless, a substantial load of colloids was transported through the entire study reach to Pueblo Reservoir. Dissolved metals were dominated by Mn and Zn, and their concentrations remained relatively high throughout the 250-km reach. The composition of extractable and total metals in bed sediment for several kilometers downstream from California Gulch is similar to the composition of the colloids that settle to the bed. Substantial concentrations of Mn and Zn were extractable, which is consistent with sediment-water chemical reaction. Concentrations of Cd, Pb, and Zn in bed sediment clearly result from the influence of mining near Leadville. Concentrations of Fe and Cu in bed sediments are nearly equal to concentrations in colloids for about 10 km downstream from California Gulch. Farther downstream, concentrations of Fe and Cu in tributary sediments mask the signal of mining inflows. These results indicate that colloids indeed influence the occurrence and transport of metals in rivers affected by mining.  相似文献   

3.
A dialysis procedure was used to assess the distribution coefficients of ∼50 major and trace elements (TEs) between colloidal (1 kDa–0.22 μm) and truly dissolved (<1 kDa) phases in Fe- and organic-rich boreal surface waters. These measurements allowed quantification of both TE partitioning coefficients and the proportion of colloidal forms as a function of solution pH (from 3 to 8). Two groups of elements can be distinguished according to their behaviour during dialysis: (i) elements which are strongly associated with colloids and exhibit significant increases of relative proportion of colloidal forms with pH increase (Al, Ba, Cd, Co, Cr, Cu, Fe, Ga, Hf, Mn, Ni, Pb, rare earth elements (REEs), Sr, Th, U, Y, Zn, Zr and dissolved organic C) and (ii) elements that are weakly associated with colloids and whose distribution coefficients between colloidal and truly dissolved phases are not significantly affected by solution pH (As, B, Ca, Cs, Ge, K, Li, Mg, Mo, Na, Nb, Rb, Sb, Si, Sn, Ti, V). Element speciation was assessed using the Visual MINTEQ computer code with an implemented NICA-Donnan humic ion binding model and database. The model reproduces quantitatively the pH-dependence of colloidal form proportion for alkaline-earth (Ba, Ca, Mg, Sr) and most divalent metals (Co, Cd, Mn, Ni, Pb, Zn) implying that the complexation of these metals with low molecular weight organic matter (<1 kDa fraction) is negligible. In contrast, model prediction of colloidal proportion (fraction of 1 kDa–0.22 μm) of Cu2+ and all trivalent and tetravalent metals is much higher than that measured in the experiment. This difference may be explained by (i) the presence of strong metal-binding organic ligands in the <1 kDa fraction whose stability constants are several orders of magnitude higher than those of colloidal humic and fulvic acids and/or (ii) coprecipitation of TE with Fe(Al) oxy(hydr)oxides in the colloidal fraction, whose dissolution and aggregation controls the pH-dependent pattern of TE partitioning. Quantitative modeling of metal – organic ligand complexation and empirical distribution coefficients corroborate the existence of two colloidal pools, formerly reported in boreal surface waters: “classic” fulvic or humic acids binding divalent transition metals and alkaline-earth elements and large-size organo-ferric colloids transporting insoluble trivalent and tetravalent elements.  相似文献   

4.
High concentrations of metals in organic matter can inhibit decomposition and limit nutrient availability in ecosystems, but the long-term fate of metals bound to forest litter is poorly understood. Controlled experiments indicate that during the first few years of litter decay, Al, Fe, Pb, and other metals that form stable complexes with organic matter are naturally enriched by several hundred percent as carbon is oxidized. The transformation of fresh litter to humus takes decades, however, such that current datasets describing the accumulation and release of metals in decomposing organic matter are timescale limited. Here we use atmospheric 210Pb to quantify the fate of metals in canopy-derived litter during burial and decay in coniferous forests in New England and Norway where decomposition rates are slow and physical soil mixing is minimal. We measure 210Pb inventories in the O horizon and mineral soil and calculate a 60-630 year timescale for the production of mobile organo-metallic colloids from the decomposition of fresh forest detritus. This production rate is slowest at our highest elevation (∼1000 m) and highest latitude sites (>63°N) where decomposition rates are expected to be low.We calculate soil layer ages by assuming a constant supply of atmospheric 210Pb and find that they are consistent with the distribution of geochemical tracers from weapons fallout, air pollution, and a direct 207Pb application at one site. By quantifying a gradient of organic matter ages with depth in the O horizon, we describe the accumulation and loss of metals in the soil profile as organic matter transforms from fresh litter to humus. While decomposition experiments predict that Al and Fe concentrations increase during the initial few years of decay, we show here that these metals continue to accumulate in humus for decades, and that enrichment occurs at a rate higher than can be explained by quantitative retention during decomposition alone. Acid extractable Al and Fe concentrations are higher in the humus layer of the O horizon than in the mineral soil immediately beneath this layer: it is therefore unlikely that physical soil mixing introduces significant Al and Fe to humus. This continuous enrichment of Al and Fe over time may best be explained by the recent suggestion that metals are mined from deeper horizons and brought into the O horizon via mycorrhizal plants. In sharp contrast to Al and Fe, we find that Mn concentrations in decomposing litter layers decrease exponentially with age, presumably because of leaching or rapid uptake, which may explain the low levels of acid extractable Mn in the mineral soil. This study quantifies how metals are enriched and lost in decomposing organic matter over a longer timescale than previous studies have been able to characterize. We also put new limits on the rate at which metals in litter become mobile organo-metallic complexes that can migrate to deeper soil horizons or surface waters.  相似文献   

5.
Changes in size distribution and elemental composition of 0.5-50 nm fresh water colloids during estuarine mixing have been studied by in-laboratory mixing of natural creek water and synthetic seawater, followed by size fractionation with Asymmetrical Flow Field-Flow Fractionation, and online elemental quantification by High-Resolution ICPMS. At least two types of colloids were present in the studied size region; 0.5-3 nm fluorescent dissolved organic matter (FDOM), and >3 nm colloids that were rich in Fe and colored dissolved organic matter (CDOM). Most trace elements were associated in different proportions to these two populations of colloids. Following mixing with synthetic seawater, the >3 nm Fe-rich colloids and CDOM were extensively removed from the studied size region by salt induced aggregation. The degree of removal with increasing salinity was greatest below 2.5‰ salinity, continued to a lesser degree between 2.5‰ and 15‰ salinity, above which only very small additional removal could be distinguished. At 25‰ salinity, the Fe concentration in the 0.5-50 size region had been reduced down to 15% of its original value in freshwater, while the amount of CDOM had been reduced to 55%. On the contrary, the concentration of the 0.5-3 nm FDOM was unchanged by the increased concentration of sea salt. Therefore, colloidally associated Al, P, Co, Cu, Zn, Ce, Lu and Pb were removed from the 0.5-50 nm size region according to their relative distributions between the FDOM and the Fe-rich colloids. Consequently, at 25‰ salinity, the 0.5-50 nm concentrations of Al, Mn, P and Pb, (mainly associated with the Fe-rich colloids) had been reduced down to 13-26 % of their values in freshwater, while the concentrations of Co and Cu (with higher preferences for FDOM) were less reduced, down to 46% and 57%, respectively. Changes in the elemental composition of the remaining colloidal matter were observed, the most pronounced were increased contents of P, Al and Pb in Fe-rich colloidal matter of medium size (∼3-15 nm) and increased Pb content in Fe-rich colloidal matter of larger size (∼5-50 nm).  相似文献   

6.
Dissolved and particulate concentrations of metals (Fe, Al, Mn, Co, Ni, Cu, Zn, Cd, Tl, Pb) and As were monitored over a 5 year period in the Amous River downstream of its confluence with a creek severely affected by acid mine drainage (AMD) originating from a former Pb–Zn mine. Water pH ranged from 6.5 to 8.8. Metals were predominantly in dissolved form, except Fe and Pb, which were in particulate form. In the particulate phase, metals were generally associated with Al oxides, whereas As was linked to Fe oxides. Metal concentrations in the dissolved and/or particulate phase were generally higher during the wet season due to higher generation of AMD. Average dissolved (size < 0.22 μm) metal concentrations (μg/L) were 1 ± 4 (Fe), 69 ± 49 (Al), 140 ± 118 (Mn), 4 ± 3 Co, 6 ± 4 (Ni), 1.3 ± 0.8 (Cu), 126 ± 81 (Zn), 1.1 ± 0.7 (Cd), 0.9 ± 0.5 (Tl), 2 ± 3 (Pb). Dissolved As concentrations ranged from 5 to 134 μg/L (30 ± 23 μg/L). During the survey, the concentration of colloidal metals (5 kDa < size < 0.22 μm) was less than 25% of dissolved concentrations. Dissolved metal concentrations were generally higher than the maximum concentrations allowed in European surface waters for priority substances (Ni, Cd and Pb) and higher than the environmental quality standards for other compounds. Using Diffusion Gradient in Thin Film (DGT) probes, metals were shown to be in potentially bioavailable form. The concentrations in Leuciscus cephalus were below the maximum Pb and Cd concentrations allowed in fish muscle for human consumption by the European Water Directive. Amongst the elements studied, only As, Pb and Tl were shown to bioaccumulate in liver tissue (As, Pb) or otoliths (Tl). Bioaccumulation of metals or As was not detected in muscle.  相似文献   

7.
Due to the importance of colloids in regulating element transport and mobility in aquifers, As distribution in the colloidal fraction needs to be identified in high As groundwaters. Groundwater samples were filtered in the field through a progressively decreasing pore size (0.45 μm, 100, 30, 10, 5 kDa) using a filtration technique under a N2 atmosphere. Major and trace elements and organic C (OC) were measured in (ultra)filtrates. The studied groundwater samples have typical physio-chemical characteristics of the basin waters. Declines in concentrations of alkali (Na, K), alkaline-earth (Mg, Ca, Sr, Ba) elements, Mo, Si and Se during ultrafiltration are smaller relative to other elements. Arsenic, Cu, Cr, U and V are generally about 30% lower in 5 kDa ultrafiltrates in comparison with 0.45 μm filtrates. Around 50% of Fe, OC and Al are bound to colloids with grain size between 5 kDa and 0.45 μm. Two types of colloids, including large-size Fe colloids and small-size organic colloids, have been identified. Results indicate that As would be more likely to be associated with small-size organic colloids than Fe colloids. SEM images and EDS analysis and synchrotron XRF analyses confirm the association of As with NOM with molecular weights of 5-10 kDa. The better correlation between As(V) and OC in the 5-10 kDa fraction indicates that the small-size organic colloids have a greater affinity for As(V) than As(III). Arsenic associated with organic complexes may not be immobilized by adsorption, and, therefore, easily transported in the aquifer. Thus, the presence of As-containing colloidal complexes in high As groundwaters must be considered in the modeling of As transport in the aquifers.  相似文献   

8.
Lanthanoids were studied in a boreal landscape where an abundance of acid sulfate soils and Histosols provide a unique opportunity to increase the understanding of how these metals behave in acidic soils and waters and interact with soil and aqueous organic matter. In the acid sulfate soils lanthanoids are mobile as reflected in high to very high concentrations in soil water and runoff (typically a few mg l−1 but up to 12 mg l−1) and abundant release by several relatively weak extractants (ammonium acetate EDTA, sodium pyrophosphate, hydroxylamine hydrochloride) applied on bulk soil. Normalisation with the lanthanoid pool in the underlying parent materials (sulphide-bearing sediments deposited in brackish-water) and soil water showed that the extensive release/retention in the acidic soil was accompanied by large, and variable, fractionation trends across the lanthanoid series. In low-order streams draining these soils, the lanthanoid concentrations were high and, as indicated by frontal ultrafiltration and geochemical modelling, largely dissolved (<1 kDa) in the form of the species LnSO4+ and Ln3+. In other moderately acidic stream waters (pH 4.3-4.6), organic complexation was predicted to be important in the <1 kDa fraction (especially for the heavy lanthanoids) and strongly dominating in the colloidal phase (1 kDa-0.45 μm). Along the main stem of a stream in focus (catchment area of 223 km2), lanthanoid concentrations increased downstream, in particular during high flows, caused by a downstream increase in the proportion of acid sulfate soils which are extensively flushed during wet periods. The geochemical models applied to the colloidal Ln-organic phase were not successful in predicting the measured fractionation patterns.  相似文献   

9.
Mine tailings are ubiquitous in the landscapes of mined areas. Metal solubilities were compared in two chemically distinct mine tailings from the old Mining District of Cartagena-La Unión (SE Spain). One of the tailings was acidic (pH 3.0) with 5400 mg/kg Zn, 1900 mg/kg As and 7000 mg/kg Pb. The other was neutral (pH 7.4) with 9100 mg/kg Zn, 5200 mg/kg Pb and 350 mg/kg As. In samples from the acidic tailings, more than 15% of the Zn and 55% of the Cd were extractable with 0.1 M NaNO3, and distilled water. In the neutral tailings, using the same reagents, less than 1% of the metals were extractable. A sequential extraction procedure revealed that the sum of the residual and the Fe oxide fractions of Cu, Zn and Pb comprised 80–95% in the acidic tailings and 70–90% in the neutral tailings. The acidic mine tailings had a higher metal solubility, resulting in more metal leaching in the short-term, but also a higher fraction of inert metal. In contrast, in the neutral tailings, the metals were evenly distributed between, oxides and the residual fraction. This implies lower metal mobility in the short-term, but that metal mobility may increase in the long-term. When applied to mine tailings, sequential extractions may provide misleading results because the strong cation exchange capacity of some extractants may induce pH changes and thereby significantly change metal solubility.  相似文献   

10.
The bioavailability of metals and their potential for environmental pollution depends not simply on total concentrations but on their chemical form. Consequently, knowledge of aqueous metal speciation is essential in investigating potential metal toxicity and mobility. Dissolved (<1 kDa), colloidal (1 kDa–0.45 μm) and particulate (>0.45 μm) size fractions of sulfate, organic C (OC) and 18 metals/metalloids were investigated in the extremely acidic Vörå River system in Western Finland, which is strongly affected by acid sulfate (AS) soils. In addition, geochemical modelling was used to predict the formation of free ions and complexes in these acidic waters. The most important finding of this study is that the very large amounts of elements known to be released from AS soils (including Al, Ca, Cd, Co, Cu, Mg, Mn, Na, Ni, Si and U) occur and can prevail mainly in toxic forms throughout acidic river systems; as free ions and/or sulfate-complexes. This has serious effects on the biota and particularly dissolved Al can be expected to have acute effects on fish and other organisms. In the study area, only the relatively forested upstream area (higher pH and contents of OC) had significant amounts of a few bioavailable elements (including Al, Cu, Ni and U) due to complexation with the more abundantly occurring colloidal OC in the upstream area. It is, however, notable that some of the colloidal/particulate metals were most likely associated with metal bearing phyllosilicates eroded from clay soils. Moreover, the mobilisation of Fe and As was small and As was predicted to be associated with Fe oxides, indicating a considerable influence of Fe oxides on the mobilisation/immobilisation processes of As. Elements will ultimately be precipitated in the recipient estuary, where the acidic metal-rich river water will gradually be diluted/neutralised with brackish seawater in the Gulf of Bothnia. According to speciation modelling, such a pH rise may first cause precipitation of Al, Cu and U together with organic matters closest to the river mouth, in line with previous sediment studies from the estuary.  相似文献   

11.
The Río Pilcomayo rises on the Cerro Rico de Potosí precious metal-polymetallic tin deposits of Bolivia, and flows in a southeasterly direction for ca. 600 km to Bolivia's southern border with Argentina. Mining of the Potosí deposits has occurred continuously since 1545, generating large quantities of waste materials in the headwater of the basin. In addition, a tailings dam breach at the Porco mine in 1996 released an estimated 235 000 m3 of tailings and fluid into the upper reaches of the Río Pilaya, the largest tributary to the Pilcomayo.Concentrations of As, Sb, Cd, Cu, Pb, Hg, Ag, Tl and Zn in contemporary channel sediments upstream of the Pilaya confluence are significantly elevated above background values. Elevated levels appear to be associated with pyrite- and other sulphide mineral-bearing tailings materials transported more than 200 km downstream of the Potosí mines. Significant downstream declines in elemental concentrations occur within 15 km, and again between 150 and 200 km, from the mines. The initial decrease in concentrations is due to the rapid dilution of nearly pure tailings effluent released to the river from milling facilities near Potosí. The latter decrease results from a combination of geomorphic processes including the storage of sediment-borne metals within the channel bed and the influx of ‘clean’ sediment from several large tributaries. Downstream of the Pilaya confluence, concentrations of Cu, Pb, Hg and Zn are only slightly elevated above background values, and Ag, Cd, Sb and Tl cannot be distinguished from background levels. These data suggest that while the Porco tailings spill may have had a significant short-term impact on sediment and water quality along the lower reaches of the Río Pilcomayo, its longer-term impacts were limited. Metals stored and eroded from alluvial deposits of historical age in upstream reaches appear to be an important source of metals to the river today. An additional, and perhaps more significant source, is the release of tailings effluent to the river from modern milling operations. The transport of these contaminants downstream of Icla (203 km from Potosí) appears to be restricted by aggradational processes occurring in the vicinity of Puente Sucre. In addition, downstream of the confluence of the Río Pilaya, inputs of large amounts of ‘clean’ sediment have caused dilution of the metal contaminants. Data from other studies where similar geomorphic processes have occurred suggest that the metals in the upper Pilcomayo may eventually be moved downvalley as the aggradational processes are reversed and channel stabilisation occurs. Thus, the most significant impacts of metal contamination may not be realised in downstream areas for decades.  相似文献   

12.
The Tinto and Odiel rivers drain 100 km from the Rio Tinto sulphide mining district, and join at a 20-km long estuary entering the Atlantic Ocean. A reconnaissance study of heavy metal anomalies in channel sand and overbank mud of the river and estuary by semi-quantitative emission dc-arc spectrographic analysis shows the following upstream to downstream ranges in ppm (μg g?1): As 3,000 to <200, Cd 30 to <0.1, Cu 1,500 to 10, Pb 2,000 to <10, Sb 3000 to <150, and Zn 3,000 to <200. Organic-rich (1.3–2.6% total organic carbon, TOC), sandysilty overbank clay has been analyzed to represent suspended load materials. The high content of heavy metals in the overbank clay throughout the river and estuary systems indicates the importance of suspended sediment transport for dispersing heavy metals from natural erosion and anthropogenic mining activities of the sulfide deposit. The organic-poor (0.21–0.37% TOC) river bed sand has been analyzed to represent bedload transport of naturally-occurring sulfide minerals. The sand has high concentrations of metals upstream but these decrease an order of magnitude in the lower estuary. Although heavy metal contamination of estuary mouth beach sand has been diluted to background levels estuary mud exhibits increased contamination apparently related to finer grain size, higher organic carbon content, precipitation of river-borne dissolved solids, and input of anthropogenic heavy metals from industrial sources. The contaminated estuary mud disperses to the inner shelf mud belt and offshore suspended sediment, which exhibit metal anomalies from natural erosion and mining of upstream Rio Tinto sulphide lode sources (Pb, Cu, Zn) and industrial activities within the estuary (Fe, Cr, Ti). Because heavy metal contamination of Tinto-Odiel river sediment reaches or exceeds the highest levels encountered in other river sediments of Spain and Europe, a detailed analysis of metals in water and suspended sediment throughout the system, and epidemiological analysis of heavy metal effects in humans is appropriate.  相似文献   

13.
Size fractionation of ~40 major and trace elements (TE) in peat soil solutions from the Tverskaya region (Russia) has been studied using frontal filtration and ultrafiltration through a progressively decreasing pore size (5, 2.5, 0.22 μm, 100, 10, 5, and 1 kD) and in situ dialysis through 6–8 and 1 kD membranes with subsequent analysis by ICP-MS. In (ultra) filter-passed permeates and dialysates of soil solutions, Fe, Al, and organic carbon (OC) are well correlated, indicating the presence of mixed organo-mineral colloids. All major anions and silica are present in “dissolved” forms passed through 1 kD membrane. According to their behavior during filtration and dialysis and association with mineral or organic components, three groups of elements can be distinguished: (i) species that are weakly affected by size separation operations and largely (>50–80%) present in the form of dissolved inorganic species (Ca, Mg, Li, Na, K, Sr, Ba, Rb, Cs, As, Mn) with some proportion of small (1–10 kD) organic complexes (Ca, Mg, Sr, Ba), (ii) biologically essential elements (Co, Ni, Zn, Cu, Cd) mainly present in the fraction smaller than 1 kD and known to form strong organic complexes with fulvic acids, and, (iii) elements strongly associated with aluminum, iron and OC in all ultrafiltrates and dialysates with 30–50% being concentrated in large (>10 kD) colloids (Ga, Y, REEs, Pb, Cd, V, Nb, Sn, Ti, Zr, Hf, Th, U). For most trace metals, the proportion in the colloidal fraction correlates with their first hydrolysis constant. This implies a strong control of negatively charged oxygen donors present in inorganic/organic colloids on TE distribution between aqueous solution and colloid particles. It is suggested that these colloids are formed during plant uptake of Al, Fe, and TE from mineral matrix of deep soil horizons and their subsequent release in surface horizons after litter degradation and oxygenation on redox or acid/base fronts. Dissolved organic matter stabilizes Al/Fe colloids and thus enhances trace elements transport in soil solutions.  相似文献   

14.
Mining/smelting wastes and reservoir sediment cores from the Lot River watershed were studied using mineralogical (XRD, SEM–EDS, EMPA) and geochemical (redox dynamics, selective extractions) approaches to characterize the main carrier phases of trace metals. These two approaches permitted determining the role of post-depositional redistribution processes in sediments and their effects on the fate and mobility of trace metals. The mining/smelting wastes showed heterogeneous mineral compositions with highly variable contents of trace metals. The main trace metal-bearing phases include spinels affected by secondary processes, silicates and sulfates. The results indicate a clear change in the chemical partitioning of trace metals between the reservoir sediments upstream and downstream of the mining/smelting activities, with the downstream sediments showing a 2-fold to 5-fold greater contribution of the oxidizable fraction. This increase was ascribed to stronger post-depositional redistribution of trace metals related to intense early diagenetic processes, including dissolution of trace metal-bearing phases and precipitation of authigenic sulfide phases through organic matter (OM) mineralization. This redistribution is due to high inputs (derived from mining/smelting waste weathering) at the water–sediment interface of (i) dissolved SO4 promoting more efficient OM mineralization, and (ii) highly reactive trace metal-bearing particles. As a result, the main trace metal-bearing phases in the downstream sediments are represented by Zn- and Fe-sulfides, with minor occurrence of detrital zincian spinels, sulfates and Fe-oxyhydroxides. Sequestration of trace metals in sulfides at depth in reservoir sediments does not represent long term sequestration owing to possible resuspension of anoxic sediments by natural (floods) and/or anthropogenic (dredging, dam flush) events that might promote trace metal mobilization through sulfide oxidation. It is estimated that, during a major flood event, about 870 t of Zn, 18 t of Cd, 25 t of Pb and 17 t of Cu could be mobilized from the downstream reservoir sediments along the Lot River by resuspension-induced oxidation of sulfide phases. These amounts are equivalent to 13-fold (Cd), ∼6-fold (Zn), 4-fold (Pb) the mean annual inputs of the respective dissolved trace metals into the Gironde estuary.  相似文献   

15.
Transport and sediment–water partitioning of trace metals (Cr, Co, Fe, Pb, Cu, Ni, Zn, Cd) in acid mine drainage were studied in two creeks in the Kwangyang Au–Ag mine area, southern part of Korea. Chemical analysis of stream waters and the weak acid (0.1 N HCl) extraction, strong acid (HF–HNO3–HClO4) extraction, and sequential extraction of stream sediments were performed. Heavy metal pollution of sediments was higher in Chonam-ri creek than in Sagok-ri creek, because there is a larger source of base metal sulfides in the ores and waste dump upstream of Chonam-ri creek. The sediment–water distribution coefficients (K d) for metals in both creeks were dependent on the water pH and decreased in the order Pb ≈ Al > Cu > Mn > Zn > Co > Ni ≈ Cd. K d values for Al, Cu and Zn were very sensitive to changes in pH. The results of sequential extraction indicated that among non-residual fractions, Fe–Mn oxides are most important for retaining trace metals in the sediments. Therefore, the precipitation of Fe(–Mn) oxides due to pH increase in downstream sites plays an important role in regulating the concentrations of dissolved trace metals in both creeks. For Al, Co, Cu, Mn, Pb and Zn, the metal concentrations determined by 0.1 N HCl extraction (Korean Standard Method for Soil Pollution) were almost identical to the cumulative concentrations determined for the first three weakly-bound fractions (exchangeable + bound to carbonates + bound to Fe–Mn oxides) in the sequential extraction procedure. This suggests that 0.1 N HCl extraction can be effectively used to assess the environmentally available and/or bioavailable forms of trace metals in natural stream sediments.  相似文献   

16.
This paper presents a hydrogeochemical modeling code HYDROS, which combines the multi-component transport model with equilibrium speciation module MINTEQA2. The processes of adsorption, aqueous speciation and mineral precipitation/dissolution are represented in the model. The numerical model uses a sequential iterative approach for solving the solute transport and the equilibrium geochemistry modules. Further the transport part is solved using an operator split approach wherein a finite volume method is used for solving the advective equations while a classical finite difference method is employed for solving the dispersive equations. The model performance is evaluated by comparing it with MINTOX for a literature problem. HYDROS is then applied to the case study of the transfer of transition metals with organic colloids in the swamp groundwater system of the experimental Nsimi watershed, representative of the humid tropical ecosystem of the South Cameroon Plateau. Field observations at the site swamp system suggest that the carbon is mainly transferred as organic colloids (i.e., dissolved organic carbon) produced by the slow biodegradation of the swamp organic matter. Using HYDROS, the behaviour of Al(III) and Fe(III) elements in the base flow system is simulated during inter rain events of a short rainy season (May–June 1996). The elemental time-series for Al, Fe, Cl, pH compare well with the simulation results. The colloids are found to have a strong impact on the mobilization and transfer of Al(III) and Fe(III), which are considered to have low mobility in weathering environment.  相似文献   

17.
Trace metals in soils may pose risks to both ecosystem and human health, especially in an urban environment. However, only a fraction of the metal content in soil is mobile and/or available for biota uptake and human ingestion. Various environmental availabilities of trace metals (Cu, Pb and Zn) in topsoil from highly urbanized areas of Hong Kong to plants, organisms, and humans, as well as the leaching potential to groundwater were evaluated in the present study. Forty selected soil samples were extracted with 0.11 M acid acetic, 0.01 M calcium chloride, 0.005 M diethylenetriaminepentaacetic acid, and simplified physiologically based extraction tests (PBET) for the operationally defined mobilizable, effectively bioavailable, potentially bioavailable, and human bioaccessible metal fractions, respectively. The metals were generally in the order of Zn > Cu ∼ Pb for both mobility (24%, 7.6%, 6.7%) and effective bioavailability (2.8%, 0.9%, 0.6%), Pb (18%) > Cu (13%) > Zn (7.4%) for potential bioavailability, and Pb (59%) ∼ Cu (58%) > Zn (38%) for human bioaccessibility. Although the variations in the different available concentrations of metals could mostly be explained by total metal concentrations in soil, the regression model predictions were further improved by the incorporation of soil physicochemical properties (pH, OM, EC). The effectively bioavailable Zn and Pb were mostly related to soil pH. Anthropogenic Pb in urban soils tended to be environmentally available as indicated by Pb isotopic composition analysis. Combining various site-specific environmental availabilities might produce a more realistic estimation for the integrated ecological and human health risks of metal contamination in urban soils.  相似文献   

18.
Transport of trace metals by natural organic matter (NOM) is potentially an important vector for trace metal incorporation in secondary cave precipitates [speleothems], yet little is known about the size distribution, speciation and metal binding properties of NOM in cave dripwaters. A hyperalkaline cave environment (ca. pH 11) was selected to provide information on colloid-metal interactions in cave waters, and to address the lack of high-pH data in natural systems in general. Colloidal (1 nm-1 μm) NOM in hyperalkaline cave dripwater from Poole’s Cavern, UK, was characterised by flow field-flow fractionation (FlFFF) coupled to UV and fluorescence detectors and transmission electron microscopy (TEM) coupled to X-ray energy-dispersive spectroscopy (X-EDS); trace-metal lability was examined by diffusive gradients in thin films (DGT). Colloidal aggregates and small particulates (>1 μm) imaged by TEM were morphologically heterogeneous with qualitative elemental compositions (X-EDS spectra; n = 41) consistent with NOM aggregates containing aluminosilicates, and iron and titanium oxides. Globular organic colloids, with diameters between ca. 1 and 10 nm were the most numerous colloidal class and exhibited high UV-absorbance (254 nm) and fluorescence intensity (320:400 nm excitation: emission) in optical regions characteristic of humic-like compounds. Metal binding with humic substances was modelled using the WHAM 6.1 (model VI) and visual MINTEQ 3.0 (NICA-Donnan) speciation codes. At pH 11, both models predicted dominant humic binding of Cu (ca. 100%) and minimal binding of Ni and Co (ca. <1-7%). A DGT depletion experiment (7 days duration) with the hyperalkaline dripwater showed that the available proportion of each metal was much lower than its total concentration. Metal availability for DGT in the initial stages (24 h) was consistent with weaker binding of alkaline earth metals by humic substances (Ba > Sr > V > Cu > Ni > Co), compared to the transition metals. Integrated over the entire experiment, the DGT-available proportion of transition metals (Ni > Cu & V >> Co) differed greatly from the expected hierarchy from WHAM and MINTEQ, indicating unusually strong complexation of Co. Total metal concentrations of Cu, Ni, and Co in raw and filtered PE1 dripwater samples (n = 53) were well correlated (Cu vs. Ni, R2 = 0.8; Cu vs. Co, R2 = 0.5) and were strongly reduced (> ca. 50%) by filtration at ca. 100 and 1 nm, indicating a common colloidal association. Our results demonstrate that soil-derived colloids reach speleothems, despite transport through a karst zone with potential for adsorption, and that NOM is a dominant complexant of trace metals in high pH speleothem-forming groundwaters.  相似文献   

19.
Arctic rivers typically transport more than half of their annual amounts of water and suspended sediments during spring floods. In this study, the Sagavanirktok, Kuparuk and Colville rivers in the Alaskan Arctic were sampled during the spring floods of 2001 to determine levels of total suspended solids (TSS) and dissolved and particulate metals and organic carbon. Concentrations of dissolved organic carbon (DOC) increased from 167 to 742 μmol/L during peak discharge in the Sagavanirktok River, at about the same time that river flow increased to maximum levels. Concentrations of dissolved Cu, Pb, Zn and Fe in the Sagavanirktok River followed trends observed for DOC with 3- to 25-fold higher levels at peak flow than during off-peak discharge. Similar patterns were found for the Kuparuk and Colville rivers, where average concentrations of dissolved trace metals and DOC were even higher. These observations are linked to a large pulse of DOC and dissolved metals incorporated into snowmelt from thawing ponds and upper soil layers. In contrast with Cu, Fe, Pb and Zn, concentrations of dissolved Ba did not increase in response to increased discharge of water, TSS and DOC. Concentrations of particulate Cu, Fe, Pb and Zn were more uniform than observed for their respective dissolved species and correlated well with the Al content of the suspended particles. However, concentrations of particulate Al were poorly correlated with particulate organic carbon. Results from this study show that >80% of the suspended sediment and more than one-third of the annual inputs of dissolved Cu, Fe, Pb, Zn and DOC were carried to the coastal Beaufort Sea in 3 and 12 d, respectively, by the Kuparuk and Sagavanirktok rivers.  相似文献   

20.
Intensive mining has taken place in the Iberian Pyrite Belt since 3000 B.C. generating Acid Mine Drainage (AMD) and releasing high amounts of SO4, acidity, metals and metalloids into surface water. Concentrations of elements in AMD-impacted waters are regulated by the precipitation of Fe-rich materials and particulate matter can influence the mobility and the bioavailability of metals. In this paper a study on the dissolved As species concentration along a polluted stream has been performed. Two sampling campaigns were conducted during the dry and the rainy seasons. Concentrations of dissolved elements are higher during the dry season and increase progressively along the water course in both seasons. Concentrations up to 80 μg L−1 of As3+ and 5 mg L−1 of As5+ were determined. The concentration of As species increases and the As3+/As5+ ratio decreases downstream. The Fe2+/Fe3+ and As3+/As5+ ratios show the same pattern with respect to pH for all the examined samples, except those taken from Au cyanidation wastes. The particulate phase is mainly composed of Fe, As and Pb, with As being associated with the Fe minerals while Pb seems to be associated with the clay colloids.  相似文献   

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